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and J. D. HUNT
Oxford, U.K.
(Rcceired 16 February
1981)
Abstract-Ceil and primary dendrite arm spacings have been measured in AI-& and Al-Mg-Si alloys
directionally solidified at steady state over a very large range of growth conditions. The Al-Mg-Si alloys
have been chosen so as to minimize gravitational fluid flow in the liquid. A spacing parameter, 1, has
been correlated with the liquid temperature gradient GL, the growth velocity, V and the bulk alloy
composition, C,.
It has been found that for dendrites in the ALMg-Si system
j.
272G;o.S
V-o.8
Cafe
INTRODUCTION
There has been considerable experimental work in the
past number of years on the measurement of cell and
primary dendrite arm spacings in a variety of alloy
systems [l-11]. Much of this has, however, been carried out under conditions in which the temperature
1851
1852
MCCARTNEY
AND
HUNT:
ALLOYS
system to make
-crucible
~=(~)c~~(~)~~
flow of solute
/rich liquid.
/isotherm
/macroscopic
S/L interface shape
during growth
EXPERIMENTAL
METHOD
Apparatus
The aluminium alloy specimens contained in
graphite crucibles were directionally solidified in three
different types of furnace arrangements in order to
cover the required ranges of growth velocity and
temperature gradient.
Low temperature gradients of between 0.2 and
1.5K mm- at growth rates ranging from 4 x 10-s
to lo- mm s-i were obtained by using a thermal
valve furnace [16] which is shown schematically in
Fig. 3. The alloy was contained in a graphite crucible
of 9.0mm O.D. and 300mm total length which was
drilled out to a depth of 180mm with an I.D. of
7.3 mm. The furnace consisted of three separate heating zones each of which was controlled independently,
and the crucible was held in a fixed position. The
MCCARTNEY
Al
AND
HUNT:
1853
At %
Si
Fig. 2. Al rich corner of the Al-Mg-Si phasq diagram showing eutcctic valleys (solid lines) and isotherms
rod. Unidirectional growth was achieved by withdrawing the specimen at a constant rate into a water
bath contained in a water-cooled brass jacket which
was inserted into the hot zone of the furnace. Preliminary experiments were carried out to check that the
withdrawal rate was qua1 to the growth rate of the
interface over the entire range of growth conditions.
control
thermocouple.
top furnace.
_ _._tirmocouDle
iiikple.
1854
MrCARTNEY
AND
HUNT:
DIRECTIONALLY
SOLIDIFIED
ALUMINIUM
ALLOYS
The
oxidation,
ducing a rapidly solidified cast rod of 10.5 mm diameter and 150 mm long. Slices of this cast rod were
chemically analyzed using atomic absorption spectrophotometry. Slices taken from either end were found
to be of slightly different composition from those
taken from the central 140 mm of the rod which were
of uniform composition and within 5% of the made
up composition. Thus 1Omm were discarded from
each end of the master alloy rod and only the central
130 mm was used in making up the Al-Mg-Si alloys.
water
bath.
minsulation.
Fig. 4. Sectional view of intermediate temperature gradient
furnace.
1
Irm
128
76
72
66
158
118
96
475
310
280
200
175
471
415
349
251
398
380
355
Morphology
D
::
::
D
::
D
D
D
D
D
D
D
:
C
C
Growth
Rate mm s-l
Liquid
temperature
gradient
K mm-
1.0
1.0
1.0
1.0
5 x 10-l
5 x 10-l
5 x 10-I
5 x 10-z
5 x 10-z
5 x 10-f
5 x lo-*
5 x 10-f
1.67 x IO-*
1.67 x IO-
1.67 x IO-*
1.67 x IO-*
4.3 x lo-
4.3 x lo-
4.3 x 1o-3
3.40
11.0
12.1
15.5
4.85
8.70
13.9
2.05
5.50
7.90
11.8
16.7
3.67
4.86
6.70
13.0
4.2
6.0
8.4
0.
MCCARTNEY
HUNT:
AND
DIRECTIONALLY
Growth rate
mms-
Liquid temperature
gradient K mm-
444
439
320
320
290
390
231
302
176
300
151
140
198
87
210
70
870
630
1034
1270
860
800
1055
1.73 x
1.73 x
1.73 x
1.73 x
1.73 x
3.30 x
5 x
6.67 x
6.67 x
4.10
5.20
9.40
9.70
11.7
4.20
9.20
4.80
14.2
3.95
14.7
17.0
3.74
14.7
2.92
15.5
1.64
1.10
1.12
1.14
0.92
0.84
0.45
10-z
10-l
1o-z
10-z
10-2
10-l
10-Z
IO-*
lo-*
10-l
10-l
10-l
5 x 10-l
5 x 10-l
1.0
1.0
1.18 x lo-*
10-I
1.45 x 10-z
7.70 x lo-
3.67 x 1O-2
6.45 x 1O-2
1.08 x 10-l
126
133
220
340
616
434
895
614
532
380
612
48.0
60.5
76.4
55.3
Morphology
Growth rate
mm s-l
Liquid
temperature
gradient
K mm-
5 x
D
M
10-l
5 x 10-l
10-l
1.05 x 10-l
1.50 x 10-l
6.91 x lo-
4.60 x 10-2
3.33 x 10-2
3.85 x lo-
3.17 x 10-z
1.83 x 1O-2
5 x 10-l
3.15
2.30
2.35
1.08
0.35
0.92
0.30
0.66
0.81
1.67
0.76
11.0
5 x 10-l
5 x 10-l
10-l
8.82
6.05
18.5
72.1
99.0
158
66.0
89.7
85.0
154
175
98.0
154
130
173
M
C
C
C
C
3.33 x
3.33 x
3.33 x
3.33 x
3.33 x
1.67 x
1.67 x
8.3 x
8.3 x
10-l
10-l
10-l
10-2
10-2
10-2
10-2
10-2
lo-
1O-2
1O-3
lo-
ALUMINIUM
ALLOYS
1855
i
/tm
C,Si
at./,
Growth rate
mms-
Liquid
temperature
gradient
K mm-
145
190
239
275
338
0.35
0.83
I .39
2.61
4.68
lo-
10-l
10-l
10-l
10-l
5.85
5.80
6.05
5.50
6.23
1
Itm
SOLIDIFIED
11.0
4.20
6.3
18.0
10.0
9.65
5.55
4.43
11.0
5.48
8.43
4.40
Al-6wt.% Cu
The measurements of the primary spacing parameter, k on A1-6 wt.% Cu are listed in Table 1 and
presented graphically in Fig. 5 in which log 1 is
plotted against log GL for various different growth
velocities Y
All the closed points represent specimens which
solidified dendritically with macroscopically planar
solid-liquid interfaces. The open points represent
those specimens which solidified with a cellular
morphology and with macroscopically curved solid
liquid interfaces. A longitudinal section through the
quenched interface of such a specimen is shown in
Fig. 6. Electron microproble analysis of this specimen
revealed that the composition of the quenched liquid
20 mm from the interface was uniform and equal to
the made up composition of 6wtP/,Cu. The composition of the quenched liquid was also analyzed just
ahead of the leading part of the macroscopic interface
and down the right hand side of the specimen. Ahead
of the leading edge it was found to contain
6.5 wt.%Cu whereas down the side the Cu content
rose to approximately 11.5 Wt.% Cu, indicating severe
segregation due to gravitational fluid flow.
A best fit double linear regression analysis on all
the data at 1.67 x lo- mm s-l and above shows
that
~ = K Gi0.55 V-o.28
where K is a constant and there is a standard error in
both exponents of f0.02. The primary spacings in
1856
MCCARTNEY
AND
HUNT:
Lyok)
DIRECTIONALLY
SOLIDIFIED
ALUMINIUM
ALLOYS
AL-6wt/oCu
2.1 2.0 -
0.2
I
03
I
0.1
I
05
1
0.6
I
0.7
I
08
I
09
I
1.0
1
14
I
1.2
-I
1.3
h(GJ
Fig. 5. Plot of log 1 vs log GLfor Al-6 wt.% Cu at various different growth velocities, I! Closed points
represent dendritic specimens. Open points represent cellular specimens solidified at V = 4.3 x lo-
mms-. Lines of slope -0.5 are drawn through the dendritic points.
Fig. 6. Longitudinal section showing the quenched interface of an AI-6 wt.,, Cu specimen with Y = 4.3 x
IO- mm s-I and GL = 5.5 K mm-. Magnification =
23 x .
In order to reduce the macroscopic interface curvature due to fluid flow (see Fig. 1) it is necessary to
eliminate, or reduce to a small value, density changes
with composition and temperature ahead of the dendrite tips and in the interdendritic liquid. This can be
done by choosing a ternary alloy containing one solute element which is denser than the solvent and one
which is less dense. If the composition of an alloy is
adjusted there will be one particular atomic ratio of
Mg to Si which just eliminates density changes with
composition and temperature along the liquidus. A
series of unidirection growth experiments was carried
out at a growth rate of 4.3 x lo- mms- with a
temperature gradient of 5.5 K mm- in order to determine the Mg to Si ratio which produced a minimal
amount of fluid flow (as assessed by the macroscopic
interface curvature of a quenched specimen).
A number of alloy specimens each containing a
known amount of solute but with different Mg to Si
ratios weie directionally frozen at steady state for approximately 50mm and rapidly quenched. A longitudinal section containing the quenched interface was
then examined and its macroscopic curvature com-
MCCARTNEY
AND
HUNT:
1857
(b)
Fig. 7. (a) Longitudinal section showing the quenched interface of an Al-Cu eutectic specimen. V = 4.3
x 10-3nuns;GL = 6.8 Kmm-. Magnification = 23 x . @)L.ongitudinal section showing the quenched
inte~a~ofanAl=0.61at.~M~l.3Qat.~gis~men.
V=4.3 x 10-mns-;
Magnification = 23 x .
GL=5.5Kmm-.
Gi0.54
V-O.8
v-0.20
1858
MCCARTNEY
AND
HUNT:
ALLOYS
WX)
t
dendrites
f-----.
Fig. 8. Plot of log A vs log (C, Y.) for cells and dendrites. Circles represent dendritic specimens, squares
cellular ones. &St fit lines are drawn through the points and a line of slope -0.5 is indicated for
comparative purposes.
are for
SUNNY
OF RESULI3
The extensive data on Al-h4gSi alloys directionally solidified at steady state vertically upwards and
stable against fluid flow give the following main
results:
(i) 1 ==346 GLO*ss Y-oP2s for dendrites grown from
alloys of composition Al-O.61 at.% Mg-1.39 at.% Si
with a standard error &0.02 in both exponents.
(ii) A = 181 Gi** Y-o.zs for dendrites grown
from alloys of composition Al - 0.15 at.% Mg - 0.33
at.%Si with standard errors of f0.03 and f0.02 in
the GL and V exponents respectively.
1 = 145 GL0*46V-o*2ofor cells grown from the
same composition with standard errors of &0.04 and
f 0.02 respectively.
MCCARTNEY
AND
HUNT:
DIRECTIONALLY
SOLlDlFIED
ALUMINIUM
ALLOYS
1859
Dendrites
f
:,a&ufvs.
+
v =3.3&&n/$.
f
4
v=W&ulvs.
v =ti?n*
Fig. 9. Plot of log 1 vs log GL for cells and dendrites grown from Al-O.15 at.% Mg-0.33 at.% Si at four
+-O-45l
-036I
-0.26
I
-096-046
t
1 0 I
I
*O-l0
,
l
I
0-x
I
+ 0-u
I
* OIL
Log(&&if
Fig. 10. Plot of log I vs log (CT,,,) at a constant temperature gradient (6 K mm-), growth rate
(lo- mm s- *), and atomic ratio of Mg to Si (0.45). A best fit line is drawn through the points and one of
slope 0.33 is included for comparison.
186@
MCCARTNEY
AND
HUNT:
DIRE~lONALLY
DISCUSSION
Comparison with theoretical models
SOLIDIFIED
ALUMINIUM
ALLOYS
transition
x
8
VCS
Al-Zwt%Cu.
io*
Fig. Ii. I as a function of Y in an Al-2 wt.% Cu alloy at a temperature gradient of IOK mm- as
predicted by the models of Hunt (241 and Kurz and Fisher [25] (Iabelled Hand K-F respectively). The
data is taken from Ref. [253, and V,, is the constitotiona1 supercooling velocity for planar front growth.
MCCARTNEY
h
AND HUNT:
SQUARE
ARRAY
.
.
DIRECTIONALLY
is the
in an area A
AL
.
.
ALUMINHJM
ALLOYS
1861
X-l;,-?KiZ
SOLlDlFIED
ARRAY
l
$=,.OKiW$
work
1862
MCCARTNEY
AND
HUNT:
DIRECTIONALLY
SOLiDPIED
ALUMINJUM
ALLOYS
(a)
Fig. 13. (a) Cell ular array in an Al-O.15 at.% Mg-0.33 at.% Si alloy. Magnification = 90x : . (b) Dendritic
array in an Al-O.63 at.% Mg-l.39at./0 Si alloy. Magnification = 75 x .
SUMMARY
AND Cf3INCLUSIONS
been obtained
in the ACMg-S i systern which exhibit little fluid flopw in the interden dritic
or bulk liquid, These have been obtained over a wide
Experimental
results
have
MCCARTNEY
AND
HUNT:
DIRECTIONALLY
range of liquid temperature gradient, GL, growth velocity, V and alloy composition, C,. The parameter A,
which is a measure of the primary arm spacing has
been related to GL, V and C, using linear regression
analyses. It has been found that for dendrites the
relationship is of the form
SOLIDIFIED
ALUMINIUM
ALLOYS
1863
(1971).
7. K. P. Young and D. H. Kirkwood. Mecull. Trans. A 6,
197 (1975).
8. T. Okamoto,
Acra metall.
REFERENCES
1. J. A. E. Bell and W. C. Winegard, J. Inst. Metals 92,
357 (1964).
2. P. K. Rohatgi and C. M. Adams, Trans. Metall. Sot.
A.I.M.E. 239, 1729, 1737 (1967).
3. J. 0. Coulthard and R. Elliott. J. Inst. Metals 95, 21
(1967).
4. R. Alberny, J. Serra and T. Turpin, Trans. Metall. Sot.
A.I.M.E. 245. 55 (19691.
5. R. E. Jesse and H. F. J. I. Gillcr, J. Cryst. Growth 7,
348 (1970).
A.I.M.E.
35. C. J. Smithells (ed.), Metals Reference Book, 5th Edition, p. 944, Butterworths (1978).